Science Advances
·
2025
·Vol. 11
·期 30
·
IF 12.5
Xinxin Li,Weiwei Zhang,Guang Miao,Zhikang Wu,Xingjie Wang,Xuan Wei,Zewei Liu,Hao Tang,Cuiting Yang,Jing Xiao
Separating perfluorinated cyclopropane/propane mixtures is critical yet challenging for sustainably producing high-purity perfluropropane in the advanced electronics industry. Conventional one-step adsorption separation methods lack proper selectivity due to similar molecular sizes and properties. We introduce a tandem reaction-adsorption approach with ultrahigh selectivity and low-pressure uptake. The initial step converts perfluorinated cyclopropane into olefins, enhancing molecular size and polarity differences and enabling efficient sieving using a scalable, stable molecular sieve developed. The method achieves selectivity over two orders of magnitude higher than conventional methods, producing 99.9999% pure perfluropropane at 12.5 liters per kilogram per hour with a 98.8% yield in the fixed beds. The tandem reaction-adsorption methodology introduces an efficient route for separating and purifying industrially challenging gas analogs.
研究领域:
化学工程
·
材料科学
·
分离技术
·
工业化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yakun Liu,Shennan Yang,Chengxiang Shi,Lun Pan,Xiangwen Zhang,Ji-Jun Zou
Simmons-Smith cyclopropanation commonly promoted by CF 3 COOH is one important method for transforming olefin into high-energy–density cyclopropyl fuel, but it brings problems such as high cost and harm to environment. In this work, a series of highly active solid acid catalysts HPW/MCM-41 is prepared by impregnation method for the cyclopropanation of dicyclopentadiene. The composition, structural and acidity of catalyst were characterized by TEM, XRD, NH 3 -TPD, etc. The 5 % HPW/MCM-41 contains more Dawson-type P 2 W 18 (H 6 P 2 W 18 O 62 ) and defective-type P 2 W 21 (H 6 P 2 W 21 O 71 ) that can provide the most abundant acid sites. This catalyst shows the best catalytic activity, the conversion and bicyclic product selectivity for cyclopropanation of dicyclopentadiene are 93.4 % and 55.7 %, respectively, both higher than that of CF 3 COOH. Moreover, such catalyst shows good catalytic activity for several olefin substrates, and can be recycled in several runs. This work provides a green and efficient catalyst for cyclopropanation reactions for synthesis of high-energy–density fuel, pesticide and medicine.
研究领域:
催化化学
·
能源化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Wei Wang,Zhensheng Shen,Jiaxiang Zhang,Lun Pan,Chengxiang Shi,Xiangwen Zhang,Ji-Jun Zou
High-energy–density fuels play a vital role in the development of the aviation industry because they can provide more propulsion energy than conventional liquid fuels. Constructing more five- or six-membered rings in fuel molecules is an efficient way to increase fuel density. However, as the number of rings increases, the hydrogen content of fuel molecules gradually decreases, resulting in a decrease in the mass calorific value, which limits the further improvement of the volumetric calorific value, meanwhile, the low-temperature characteristics of the fuel become worsen. Considering the high strain energy stored in cyclopropane moiety and the good cryogenic properties of spiro fuel, in this work, two spirocyclopropane high-energy–density fuels have been synthesized from cyclopentadiene by phase transfer catalytic cyclopropanation and palladium catalytic cyclopropanation, and the reaction conditions have been optimized. The synthesized fuels possess heat value and specific impulse higher than the widely used high-energy–density fuel JP-10. Additionally, their kinematic viscosity at low temperatures is only about one-third that of JP-10. The outstanding properties of the synthesized strained fuels suggest their good potential as high-energy–density fuels.
研究领域:
化学
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材料科学
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航空航天工程
·
燃料技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2020
·
IF 3.871
Sa Wang,Yufan Zhang,Yuning Tang,Yijing Wen,Zhenqiang Lv,Sihao Liu,Xiang Li,Xin Zhou
Separating propane from propylene is a significant challenge in petrochemical industry. Rational chemistry design of the propane-selective adsorbent has not been reported. This work demonstrates the first design of propane-selective adsorbents. Two strategies based on surface chemistry tuning, namely compositing 2D g-C 3 N 4 and replacing ligand, have been proposed to yield the propane-selective g-C 3 N 4 @Zr-BPDC (BPDC = biphenyl-4,4′-dicarboxylate) and Zr-BPYDC (2,2′-bipyridine 5,5′-dicarboxylate). Whereas g-C 3 N 4 @Zr-BPDC has a high propane capacity of 8.79 mmol/g at room temperature and ambient pressure, Zr-BPYDC exhibits superior propane/propylene selectivity. The isosteric heat of propane and propylene adsorption on both adsorbents is lower than that of most reported adsorbents, indicating facile regeneration of the adsorbents. DFT calculations suggest the propane-selectivity comes from multiple C H δ+ ⋯N δ− interactions between propane and nitrogen atoms of the adsorbents. Moreover, both adsorbents produce polymer-grade propylene through a one-step separation using a packed column, facilitating the energy-effective production of polymer grade propylene under ambient conditions.
研究领域:
化学工程
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材料科学
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吸附技术
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石油化学
✓ 已验证
产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2020
·Vol. 130
·期 1
·241-256
·
IF 1.52
Ge Meng,Chen Xingye,Li Yanyong,Wang Jiameng,Xu Yanhong,Zhang Lihong
This paper describes the synthesis and application of γ -Al 2 O 3 supported SmCoO 3 perovskite-type oxide in the catalytic propane dehydrogenation to propene. Various techniques including X-ray diffraction (XRD), H 2 temperature-programmed reduction (H 2 -TPR), transmission electron microscopy (TEM), thermogravimetric analysis (TG) and X-ray photoelectron spectra (XPS) were used to characterize the physico-chemical properties of SmCoO 3 /Al 2 O 3 and derived Co-based catalyst. The characterization results reveal that the perovskite lattice confinement can lead to better dispersed cobalt oxide and restrain the reduction to metallic Co species. Under the high weight hourly space velocity (3 h −1 ), the propane conversion and propene selectivity of the reduced SmCoO 3 /Al 2 O 3 catalyst were 25% and 94%, respectively, and obviously higher than those of the reduced SmCoO/Al 2 O 3 catalyst used as a referential sample prepared by an incipient wetness impregnation method. A large amount of coke was formed over the used SmCoO/Al 2 O 3 catalyst. Instead, the SmCoO 3 /Al 2 O 3 -derived Co-based catalyst can greatly reduce the amount of coke deposition. The superior catalytic performance and anti-coking ability of SmCoO 3 /Al 2 O 3 catalyst are attributed to the formation of a large amount of well-dispersed surface Co 2+ species, especially small CoO nanoparticles, and the absence of metallic Co species.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2015
·
IF 3.091
Guangren Yu,Lin Zhang,Ibrahim A. Alhumaydhi,Ahmed A. Abdeltawab,Abdulaziz A. Bagabas,Hamid A. Al-Megren,Salem S. Al-Deyab,Xiaochun Chen
Ionic liquids (ILs) coupled with Ag + or Cu + salts to form a new kind of reactive absorbent have been studied to separate light olefin from paraffin recently. In this work, we prepared two halogen-free alkylimidazolium thiocyanate ILs with cheaper cuprous thiocyanate, i.e., [Bmim]SCN–CuSCN and [Emim]SCN–CuSCN (Bmim, 1-butyl-3-methylimidazolium; Emim, 1-ethyl-3-methylimidazolium) and investigated their absorption capability for propylene, propane and mixture of both at 1–7 bar and 298–318 K. The effects of operating parameter including cation nature, temperature, pressure, Cu + concentration and reuse of absorbent were investigated. Propylene shows a chemical absorption while propane does a physical one, and increasing Cu + concentration effectively improves the absorption capability for propylene and the selectivity of propylene/propane. [Bmim]SCN–CuSCN has higher absorption capability and selectivity for propylene than [Emim]SCN–CuSCN, e.g., [Bmim]SCN–CuSCN-1.5 M can absorb 0.12 mol of propylene per liter while 0.012 mol of propane per liter at 1 bar and 298 K, with a selectivity of 10, which is comparable to some other ILs-Ag + salts and better than pure ILs. Such absorbents can be regenerated through temperature and pressure swing without remarkable activity loss. This work shows that alkylimidazolium thiocyanate ILs with Cu + salts are promising reactive absorbents to separate propylene from propane.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
iScience
·
2023
·
IF 5.8
Dake Zhang,Shenghua Wang,Xingyu Lu,Chengcheng Zhang,Kai Feng,Le He,Hui Zhang,Wei Sun,Deren Yang
Oxidative dehydrogenation of propane (ODHP) is a promising process for producing propene. Recently, some boron-based catalysts have exhibited excellent olefin selectivity in ODHP. However, their complex synthetic routes and poor stability under high-temperature reaction conditions have hindered their practical application. Herein, we report a self-evolution method rather than conventional assembly approaches to acquire structures with excellent stability under a high propane conversion, from a single precursor-MgB 2 . The catalyst feasibly prepared and optimized exhibited a striking performance: 60% propane conversion with a 43.2% olefin yield at 535°C. The BO x corona pinned by the strong interaction with the borate enabled zero loss of the high conversion (around 40%) and olefins selectivity (above 80%) for over 100 h at 520°C. This all-in-one strategy of deriving all the necessary components from just one raw chemical provides a new way to synthesize effective and economic catalysts for potential industrial implementation.
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xinyi Chen,Xin Tian,Chaohe Zheng,Haibo Zhao
Propane dehydrogenation is an attractive alternative for propylene production to petroleum-based routes. However, overcoming deactivation and toxicity of catalysts in propane direct dehydrogenation (PDH), and over oxidation in oxidative dehydrogenation (ODHP) remain challenging. Here, a chromium-based catalyst supported on a Ce-Zr solid solution is constructed for chemical looping oxidative propane dehydrogenation (CL-ODHP). A dual modulation of oxygen species by Zr doping was unraveled by characterizations and DFT calculation: the oxygen of surface CrO x was constrained while the oxygen mobility of the Ce-Zr support was promoted. Based on these properties, the interaction between surface CrO x and the support further enables an oxygen “donor–acceptor”, which potentially functions as in situ activation and regeneration of redox CrO x species as well as blockage of non-selective oxygen released from the Ce-Zr support. The optimized material (7.5Cr/Ce 0.8 Zr 0.2 O 2 ) achieves propane conversion up to 50% and propylene yield of 31% at 600 °C, and has the lowest Cr content among previously reported Cr-based catalysts that have comparable performance. These results provide insights for the design of highly active and selective redox catalysts for chemical looping as a reaction engineering strategy for the upgrading of propane dehydrogenation processes.
研究领域:
催化
·
化学工程
·
材料科学
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 15
·5930
·
IF 4.6
Xuan Wang,Wei Liang,Changqing Lin,Tie Zhang,Jing Zhang,Nan Sheng,Zhaoning Song,Jie Jiang,Bing Sun,Wei Xu
Propane catalytic oxidation is an important industrial chemical process. However, poor activity is frequently observed for stable C–H bonds, especially for non-noble catalysts in low temperature. Herein, we reported a controlled synthesis of catalyst Co3O4@CeO2–IE via inverse loading and proposed a strategy of oxygen vacancy for its high catalytic oxidation activity, achieving better performance than traditional supported catalyst Co3O4/CeO2–IM, i.e., the T50(temperature at 50% propane conversion) of 217 °C vs. 235 °C and T90(temperature at 90% propane conversion) of 268 °C vs. 348 °C at the propane space velocity of 60,000 mL g−1h−1. Further investigations indicate that there are more enriched oxygen vacancies in Co3O4@CeO2–IE due to the unique preparation method. This work provides an element doping strategy to effectively boost the propane catalytic oxidation performance as well as a bright outlook for efficient environmental catalysts.Keywords:propane catalytic oxidation;inverse loading;oxygen vacancy
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
PubMed
高影响因子
Separations
·
2022
·Vol. 9
·期 3
·64
·
IF 3.344
Weibin Cai,Jiangyu Xie,Jingyu Luo,Xiaohan Chen,Mingqian Wang,Yujun Wang,Jiding Li
In this study, zeolite molecular sieve SAPO-34/polydimethylsiloxane (PDMS) mixed matrix membranes (MMMs) were prepared to recover propane. n-Octyltrichlorosilane (OTCS) was introduced to improve compatibility between SAPO-34 and PDMS, and enhance the separation performance of the MMMs. Physicochemical properties of the MMMs were characterized by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD) and water contact angle (WCA). Results showed that, after modification, alkyl chains were successfully grafted onto SAPO-34 without changing its crystal structure, particles in the MMMs were evenly distributed in the base film, and the hydrophobicity of the MMMs was enhanced. Moreover, the effects of SAPO-34 filling content, operating pressure, and feed gas concentration on the separation performance was explored. This indicated that the modification with OTCS effectively enhanced the separation performance of SAPO-34/PDMS MMMs. When the filling content of modified SAPO-34 was 15%, the maximal separation factor of 22.1 was achieved, and the corresponding propane permeation rate was 101 GPU.Keywords:MMMs;SAPO-34;PDMS;OTCS;propane recovery
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yong Wang,Xuanyu Zhao,Shaoxiong Han,Yongzhen Wang
The development of efficient technology for natural gas separation in industrial processes has become imperative. In this regard, the exploration of novel and effective adsorbents has gained significant attention. One promising approach is the metal regulation of metal–organic frameworks (MOFs), particularly heterometallic MOFs, which offer greater potential for gas separation due to their diverse composition. This study presents the synthesis of a series of iron- and vanadium-based heterometallic MOFs (MIL-126), featuring interpenetrated structures, and investigates their adsorption performance for methane (CH4), ethane (C2H6), and propane (C3H8). Experimental results reveal that the choice of metal combinations within the MOF framework significantly influences the adsorption performance of MIL-126. Notably, heterometallic MIL-126(Fe/Ni) exhibits a stronger binding affinity for C3H8, with an impressive uptake of 177 cm3/g. The C3H8/CH4 ideal adsorbed solution theory selectivity of MIL-126(Fe/Ni) surpasses that of MIL-126(Fe) by a factor of 7, reaching a value of 853, second only to the highest reported value. Furthermore, MIL-126(Fe/Ni) exhibits remarkable potential for the recovery of pure CH4 from the equimolar C3H8/CH4 mixture, with the amount of pure CH4 approaching the maximum reported value for MOFs. Insights from isosteric heat at zero loading and Henry’s coefficients indicate that the transformation of metal types leads to a change in the interaction energy between C3H8 and the framework. Furthermore, breakthrough experiments validate the effective separation capability of MIL-126(Fe/Ni) for CH4/C2H6/C3H8 mixtures. These findings underscore the remarkable potential of heterometallic MOFs in constructing a wide range of new MOFs with tailorable properties, thereby enhancing their gas separation performance.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science China-Materials
·
2022
·Vol. 66
·期 3
·1062-1070
·
IF 8.64
Wang Yang,Chen Sai,Sun Jiachen,Xie Yufei,Zhao Zhi-Jian,Pei Chunlei,Gong Jinlong
Supported vanadium oxides (VO x ) are alternative candidates for non-oxidative propane dehydrogenation (PDH) owing to their competitive performance. This paper describes the roles of V−O sites on PDH over monomeric VO x species supported on ZrO 2 , Al 2 O 3 and SiO 2 . With the control of pre-reduction, stable structures of V−O sites are obtained for PDH, including V−O-support (V−O−S), V−OH and V=O sites. By tuning the V densities over individual support, the propylene formation rate shows a linear correlation with the number of the V−O−S site, which indicates the V−O−S site plays a decisive role in PDH rather than V−OH and V=O sites. Moreover, the specific activity per V−O−S site over ZrO 2 (8.2 × 10 −3 s −1 ) is higher than those over Al 2 O 3 (6.7 × 10 −3 s −1 ) and SiO 2 (2.8 × 10 −3 s −1 ), due to the discrepant Lewis acidity of various V−O−S sites. This research provides a fundamental insight into the intrinsic nature of V−O sites for non-oxidative propane dehydrogenation.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）